Effect of polymer–nanoparticle interactions on solvent-driven infiltration of polymer (SIP) into nanoparticle packings: a molecular dynamics study

Venkatesh, R.; Zhang, Tianren; Manohar, Neha; Stebe, Kathleen J.; Riggleman, Robert A.; Lee, Daeyeon

doi:10.1039/c9me00148d

Cited by 10 publications

(13 citation statements)

References 53 publications

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“…Future work will focus on probing how tuning the strength of the polymer–surface interaction impacts the dynamics of infiltration in the SIP system and the final extent of infiltration. Molecular dynamics simulations on the SIP system have found that by inducing stronger adhesion between the polymer and NP, a transition from dissolution-dominated infiltration to adhesion-dominated infiltration occurs . Our future work will probe experimentally how altering the nature of the surface interactions affects the extent of infiltration and the infiltration dynamics.…”

Section: Discussionmentioning

confidence: 92%

“…Molecular dynamics simulations on the SIP system have found that by inducing stronger adhesion between the polymer and NP, a transition from dissolution-dominated infiltration to adhesion-dominated infiltration occurs. 45 Our future work will probe experimentally how altering the nature of the surface interactions affects the extent of infiltration and the infiltration dynamics. To better understand partitioning and kinetics in such systems, an entropic barrier model using self-consistent field theory simulations is currently being investigated.…”

Section: ■ Conclusionmentioning

confidence: 99%

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Effect of Confinement on Solvent-Driven Infiltration of the Polymer into Nanoparticle Packings

2020

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Nanocomposite films containing a high volume fraction (>50 vol %) of nanoparticles (NPs) in a polymer matrix are promising for their functionality and use as structural coatings and also provide a unique platform to understand polymer behavior under strong confinement. Previously, we developed a novel technique to fabricate such nanocomposites at room temperature using solvent-driven infiltration of polymer (SIP) into NP packings. In the SIP process, a bilayer made of an underlying polymer film and a dense packing of NPs is exposed to solvent vapor which induces condensation of the solvent into the voids of the packing. The condensed solvent plasticizes the underlying polymer film, inducing polymer infiltration into the solventfilled voids in the NP packing. In this work, we study the effect of confinement on the kinetics of SIP and the final partitioning of the polymer into the interstices of the NP packing. We find that, while the dynamics of infiltration during SIP are strongly dependent on confinement, the final extent of infiltration is independent of confinement. The time for infiltration obeys a power law with confinement, as defined by the ratio of the chain size and the pore size. Qualitatively, the observed time scale is attributed to changes in concentration regimes as infiltration proceeds, which lead to shifting characteristic length scales in the system over time. When the concentration in the pore exceeds the critical overlap concentration, the characteristic length scale of the polymer is no longer that of the entire chain but rather the correlation length, which is smaller than the pore size. Therefore, at long times, the extent of infiltration is independent of the confinement ratio. Furthermore, favorable surface interactions between the polymer and the NPs enhance partitioning into the NP packing.

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Section: Discussionmentioning

confidence: 92%

Section: ■ Conclusionmentioning

confidence: 99%

Effect of Confinement on Solvent-Driven Infiltration of the Polymer into Nanoparticle Packings

2020

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“…suggest, the imbibition proceeds as an adhesion‐dominated process whereby the polymers move into the pores as a diffuse front of polymer chains progressing at different rates. [ 53 ] However, the authors suggest that the speed of infiltration is considerably slower for large polymers. This leaves the question of how the pore structure influences important parameters such as the surface tension and viscosity of the imbibed liquid.…”

Section: Resultsmentioning

confidence: 99%

Highly porous nanocoatings tailored for inverse nanoparticle‐polymer composites

et al. 2020

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A novel nanoparticle‐polymer composite is proposed, named inverse nanocomposites in this work. First, a rigid percolating scaffold of nanoparticles is formed, which is filled with a matrix and then polymerized. Targeted for use in thin‐film applications, these mesoporous nanoparticle scaffolds are prepared by combining the sol–gel chemistry of functionalized silanes with nanoparticles in dispersions. The nanoparticle coatings have high porosity, low density, good adhesion to the substrate, and interesting non‐classical properties, such as absorbency of highly viscous fluids. The porosity, which can be adjusted by changing the composition and preparation parameters, reaches 75%. The porous scaffold can be infiltrated with various fluids, including acrylic and epoxy monomers and even highly viscous pressure‐sensitive adhesives. If the monomers are polymerized after imbibition, the inverse nanocomposite is formed, consisting of a percolating particle network surrounded by a polymeric binder. Hence, the morphology comprises an interpenetrating system of two co‐continuous phases and not merely particles dispersed in a polymeric phase, as is typical for conventionally prepared nanocomposites.

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“…New preparation modes were recently reported to overcome the various limitations seen in conventional blending regarding the arbitrary distribution of nanoparticles in the polymer matrix, namely vapor condensation, capillary rise infiltration and ink-jetting. [6,7,[11][12][13][14] One of these new methods is based on the preparation of a highly porous nanoparticle scaffold formed by flame spray pyrolysis (FSP) [15] and the infiltration of the pores with a photo-curable monomer. [16] In a second step, the monomer is photo-polymerized under preservation of the initial particle network, forming an inverse NPC.…”

Section: Graphical Abstract Introductionmentioning

confidence: 99%

In situ polymerization monitoring of a diacrylate in an electrically conducting mesoporous nanoparticle scaffold

2022

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The properties of nanoparticle–polymer composites strongly depend on the network structure of the polymer matrix. By introducing nanoparticles into a monomer (solution) and subsequently polymerizing it, the formation of the polymer phase influences the mechanical and physicochemical properties of the composite. In this study, semi-conducting indium tin oxide (ITO) nanoparticles were prepared to form a rigid nanoparticle scaffold in which 1,6-hexanediol diacrylate (HDDA), together with an initiator for photo-polymerization, was infiltrated and subsequently polymerized by UV light. During this process, the polymerization reaction was characterized using rapid scan Kubelka–Munk FT-IR spectroscopy and compared to bulk HDDA. The conductivity change of the ITO nanoparticles was monitored and correlated with the polymerization process. It was revealed that the reaction rates of the radical initiation and chain propagation are reduced when cured inside the voids of the nanoparticle scaffold. The degree of conversion is lower for HDDA infiltrated into the mesoporous ITO nanoparticle scaffold compared to purely bulk-polymerized HDDA. Graphical abstract

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Effect of polymer–nanoparticle interactions on solvent-driven infiltration of polymer (SIP) into nanoparticle packings: a molecular dynamics study

Abstract: Dynamics of polymer motion into solvent-filled interstices of nanoparticle packings can be controlled by tuning the polymer–nanoparticle interactions, whose effect on the rate of infiltration is non-monotonic as shown by MD simulations.

Cited by 10 publications

References 53 publications

Effect of Confinement on Solvent-Driven Infiltration of the Polymer into Nanoparticle Packings

Effect of Confinement on Solvent-Driven Infiltration of the Polymer into Nanoparticle Packings

Highly porous nanocoatings tailored for inverse nanoparticle‐polymer composites

In situ polymerization monitoring of a diacrylate in an electrically conducting mesoporous nanoparticle scaffold

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